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REVIEW Overview of transient liquid phase and partial transient liquid phase bonding Grant O. Cook III Carl D. Sorensen Received: 19 January 2011 / Accepted: 12 April 2011 / Published online: 7 May 2011 Ó Springer Science+Business Media, LLC 2011 Abstract Transient liquid phase (TLP) bonding is a rel- atively new bonding process that joins materials using an interlayer. On heating, the interlayer melts and the inter- layer element (or a constituent of an alloy interlayer) dif- fuses into the substrate materials, causing isothermal solidification. The result of this process is a bond that has a higher melting point than the bonding temperature. This bonding process has found many applications, most nota- bly the joining and repair of Ni-based superalloy compo- nents. This article reviews important aspects of TLP bonding, such as kinetics of the process, experimental details (bonding time, interlayer thickness and format, and optimal bonding temperature), and advantages and disad- vantages of the process. A wide range of materials that TLP bonding has been applied to is also presented. Partial transient liquid phase (PTLP) bonding is a variant of TLP bonding that is typically used to join ceramics. PTLP bonding requires an interlayer composed of multiple lay- ers; the most common bond setup consists of a thick refractory core sandwiched by thin, lower-melting layers on each side. This article explains how the experimental details and bonding kinetics of PTLP bonding differ from TLP bonding. Also, a range of materials that have been joined by PTLP bonding is presented. Transient liquid phase (TLP) bonding Transient liquid phase (TLP) bonding is a joining process that was developed to improve upon existing bonding technologies. Specifically, this process was patented by Paulonis et al. in 1971 [1] to overcome deficiencies of then current bonding techniques in joining Ni-based superalloys [26]. TLP bonding’s main advantage is that resulting bonds have a higher melting point than the bonding tem- perature. This bonding process characteristically lies between diffusion bonding and brazing—for this reason, it is commonly called diffusion brazing. The process is also referred to by names such as transient insert liquid metal bonding [7] and is sometimes mistakenly referred to as diffusion bonding (which by definition relies solely on solid-state diffusion). See reference [8] for a detailed his- tory of TLP bonding and its many names. TLP bonding process The TLP bonding process involves the following steps: setting up the bond heating to the specified bonding temperature to produce a liquid in the bond region holding the assembly at the bonding temperature until the liquid has isothermally solidified due to diffusion homogenizing the bond at a suitable heat-treating temperature. Bond setup usually consists of placing a thin interlayer between the substrates, but the interlayer material is occasionally placed outside the joint to flow in by capil- larity [6, 7, 915] as is done in many brazing processes. The interlayer material can be in many different formats: thin foil (rolled sheet) [24, 7, 1662] amorphous foil (melt-spun) [7, 5884] fine powders (with or without binding agent) [5, 7, 1517, 8598] G. O. Cook III (&) C. D. Sorensen Ira A. Fulton College of Engineering and Technology, Brigham Young University, 435 CTB, Provo, UT 84604, USA e-mail: [email protected] 123 J Mater Sci (2011) 46:5305–5323 DOI 10.1007/s10853-011-5561-1

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  • REVIEW

    Overview of transient liquid phase and partial transient liquidphase bonding

    Grant O. Cook III • Carl D. Sorensen

    Received: 19 January 2011 / Accepted: 12 April 2011 / Published online: 7 May 2011

    � Springer Science+Business Media, LLC 2011

    Abstract Transient liquid phase (TLP) bonding is a rel-

    atively new bonding process that joins materials using an

    interlayer. On heating, the interlayer melts and the inter-

    layer element (or a constituent of an alloy interlayer) dif-

    fuses into the substrate materials, causing isothermal

    solidification. The result of this process is a bond that has a

    higher melting point than the bonding temperature. This

    bonding process has found many applications, most nota-

    bly the joining and repair of Ni-based superalloy compo-

    nents. This article reviews important aspects of TLP

    bonding, such as kinetics of the process, experimental

    details (bonding time, interlayer thickness and format, and

    optimal bonding temperature), and advantages and disad-

    vantages of the process. A wide range of materials that

    TLP bonding has been applied to is also presented. Partial

    transient liquid phase (PTLP) bonding is a variant of TLP

    bonding that is typically used to join ceramics. PTLP

    bonding requires an interlayer composed of multiple lay-

    ers; the most common bond setup consists of a thick

    refractory core sandwiched by thin, lower-melting layers

    on each side. This article explains how the experimental

    details and bonding kinetics of PTLP bonding differ from

    TLP bonding. Also, a range of materials that have been

    joined by PTLP bonding is presented.

    Transient liquid phase (TLP) bonding

    Transient liquid phase (TLP) bonding is a joining process

    that was developed to improve upon existing bonding

    technologies. Specifically, this process was patented by

    Paulonis et al. in 1971 [1] to overcome deficiencies of then

    current bonding techniques in joining Ni-based superalloys

    [2–6]. TLP bonding’s main advantage is that resulting

    bonds have a higher melting point than the bonding tem-

    perature. This bonding process characteristically lies

    between diffusion bonding and brazing—for this reason, it

    is commonly called diffusion brazing. The process is also

    referred to by names such as transient insert liquid metal

    bonding [7] and is sometimes mistakenly referred to as

    diffusion bonding (which by definition relies solely on

    solid-state diffusion). See reference [8] for a detailed his-

    tory of TLP bonding and its many names.

    TLP bonding process

    The TLP bonding process involves the following steps:

    • setting up the bond• heating to the specified bonding temperature to produce

    a liquid in the bond region

    • holding the assembly at the bonding temperature untilthe liquid has isothermally solidified due to diffusion

    • homogenizing the bond at a suitable heat-treatingtemperature.

    Bond setup usually consists of placing a thin interlayer

    between the substrates, but the interlayer material is

    occasionally placed outside the joint to flow in by capil-

    larity [6, 7, 9–15] as is done in many brazing processes.

    The interlayer material can be in many different formats:

    • thin foil (rolled sheet) [2–4, 7, 16–62]• amorphous foil (melt-spun) [7, 58–84]• fine powders (with or without binding agent) [5, 7, 15–

    17, 85–98]

    G. O. Cook III (&) � C. D. SorensenIra A. Fulton College of Engineering and Technology, Brigham

    Young University, 435 CTB, Provo, UT 84604, USA

    e-mail: [email protected]

    123

    J Mater Sci (2011) 46:5305–5323

    DOI 10.1007/s10853-011-5561-1

  • • powder compact (made by sintering, cold isostaticpressing, etc.) [57, 99–101]

    • brazing paste [9, 17, 102–104]• a physical vapor deposition process such as sputtering

    [7, 18–21, 62–64, 105]

    • electroplating [10, 17–19, 30, 88, 106–112]• evaporating an element out of the substrate material to

    create a ‘‘glazed’’ surface [113].

    A pressure is usually applied to the bonding assembly to

    keep the substrates aligned and to promote bonding; specific

    pressures are categorized in Table 1 by their nearest order

    of magnitude. For example, pressures in the nearest order

    range of 10 MPa [log(10) = 1] lie between 3.1623 MPa

    [log(3.1623) = 0.5] and 31.623 MPa [log(31.623) = 1.5].

    Occasionally, the substrates are held a fixed distance apart

    rather than applying a pressure, but this tends to cause

    porosity in the final bond [6, 19, 43].

    Heating of the bond assembly and homogenizing of the

    bond is performed with many different equipment setups

    and can occur by the following methods:

    • radiation [4, 7, 16, 17, 20, 37–43, 77–80, 105, 109, 113,122, 124, 130, 135–138]

    • conduction [35–37, 83, 95, 129]• radio-frequency induction [3, 7, 11, 21–24, 60–63, 71–

    76, 108, 110, 125–127, 129, 139–141]

    • resistance [46, 69, 100, 110]• laser [31]• infrared [7].

    The bonding process is usually confined in a vacuum [3–

    5, 7, 12, 14–17, 20–30, 35, 38–40, 46–58, 61–63, 65, 66,

    68–72, 76–83, 86–88, 93–100, 103–105, 108, 110, 112–

    115, 117, 119, 122–127, 130, 132–138, 140–157], although

    an inert atmosphere, such as argon, can be used [6, 11, 14,

    32, 33, 43, 45, 60, 67, 74, 75, 90, 111, 121, 134, 158, 159].

    On rare occasions, TLP bonding is performed under a

    different atmosphere, such as nitrogen [44], hydrogen

    [160], nitrogen and hydrogen [18], or open air [129]. The

    vacuum pressures used in the experiments referenced

    above are normally distributed about 0.1 lmHg (millitorr)with minimum and maximum values of 0.00015 and

    34 lmHg, respectively.

    TLP bonding kinetics

    TLP bonding kinetics are generally divided into the fol-

    lowing discrete stages [2, 8, 25, 56, 62, 86, 90, 99, 105,

    138, 141, 157, 161, 162] for ease of comprehending and

    modeling the process:

    • melting of the interlayer• dissolution of the substrate material• isothermal solidification• homogenization of the bond region.

    Figure 1 is a schematic of TLP bonding kinetics for a

    binary system with complete solid solubility.1 The con-

    centration profiles in the lower part of the figure are

    numbered according to the current temperature of the bond,

    which is shown in the phase diagram above them. The

    following analysis assumes that (1) the interlayer and

    substrate materials are pure elements (2) the bond region

    has a uniform temperature as it is being heated (3) the

    diffusion rates of liquid metals are infinite, and (4) the

    substrate melts back and solidifies as a plane. The second

    assumption is likely true since the interlayer is quite thin

    and generally composed of metallic elements that charac-

    teristically have moderate to high thermal conductivities.

    The third assumption is based on liquid diffusivity data

    often being orders of magnitude greater than solid diffu-

    sivity data [163]. The fourth assumption is necessary to

    characterize the process in one dimension.

    Concentration profile 1 (CP1) in Fig. 1 shows the TLP

    bonding setup at room temperature. The interlayer element

    (i) is sandwiched between two pieces of the substrate

    material element (s). The thickness of the bond region in

    Table 1 Fixturing pressures used during TLP bonding

    Nearest order Freq. (%) References

    1 kPa 8 [89, 93, 98, 114–116]

    10 kPa 5 [66, 117–119]

    100 kPa 16 [23–25, 33, 61, 68, 72, 88, 90, 99, 113, 120]

    1 MPa 36 [3, 21, 22, 26, 27, 29–31, 34, 65, 69–71, 73, 97, 102, 103, 121–128]

    10 MPa 31 [17, 28, 32, 35, 59, 60, 62–64, 67, 74, 94–96, 100, 110, 111, 129–133]

    100 MPa 4 [110, 112, 134]

    1 A numerical model was developed to calculate one-dimensional

    solid-state diffusion in conjunction with a liquid region that expands

    or contracts, assuming infinite diffusivity for the liquid region. The

    model also accounts for a heating period and diffusivity data as a

    function of concentration and temperature. Diffusivity data along with

    solidus and liquidus profiles for a hypothetical binary system were

    used to output concentration profiles that were the basis for the

    concentration profiles in Figs. 1, 3, 5, and 6.

    5306 J Mater Sci (2011) 46:5305–5323

    123

  • Fig. 1 has been exaggerated to display changes in the

    concentration profile. The interlayer can be composed of a

    single element, an alloy, or a multi-layer combination of

    elements and/or alloys.

    Interlayer thicknesses for TLP bonding are summarized

    in Table 2. Besides the frequency of each range, common

    thicknesses are also included for those ranges derived from

    at least ten references. These common thicknesses com-

    prise at least one-third of the specified range and include

    plus or minus two percent to account for differences

    between metric and English units (e.g., 0.004 inches equals

    101.6 lm and should be categorized with 100 lm). Themost common interlayer thickness is 50 lm, comprisingalmost 90% of the 40–60 lm range, or about 20% of allreported TLP bond thicknesses.

    As the bond assembly is heated, the interlayer begins to

    diffuse into the substrate materials (CP2). The amount of

    diffusion that occurs is dependent upon the interdiffusion

    coefficient between the substrate and interlayer materials as

    well as the heating rate.

    Melting

    Upon reaching the interlayer element’s melting point

    (CP3), the pure portion of the interlayer liquefies (L).

    Heating of the bond region continues until the bonding

    temperature has been reached. The bonding temperature is

    usually well above the interlayer’s melting point to ensure

    complete melting of the interlayer and to increase the rate

    of diffusion (see Optimal bonding temperature).

    CP5a

    CP4

    CP5e

    CP3

    CP5d

    CP2

    CP5c

    CP1

    CP5b

    is s

    L

    L

    L

    L

    c4,Lc4,S

    c5,Lc5,S

    c5,S

    c5,F

    c5,P

    c5,Lc5,S

    bond region

    ci0 100

    T5

    TR,P

    TR,F

    T4

    T3

    T2

    T1

    c5,Lc4,L

    c5,Sc4,S

    c5,Pc5,F

    Fig. 1 A schematic binarysystem with complete solid

    solubility and associated

    concentration profiles. These

    profiles illustrate the interlayer

    element’s concentration during

    the TLP bonding process

    J Mater Sci (2011) 46:5305–5323 5307

    123

  • Dissolution

    During heating past the melting point, the concentrations of

    the liquid region follow the solidus (c4,S) and liquidus (c4,L)

    lines of the phase diagram (CP4). This causes the liquid

    region to melt back, or dissolve, the substrate material to

    conserve mass. The movement of the solid–liquid interface

    continues until the bonding temperature has been reached

    (CP5a); at this point the liquid has attained its maximum

    width and has consumed some of the diffused solute. The

    amount of melt-back is dependent upon the solidus (c5,S)

    and liquidus (c5,L) compositions for the given material

    system at the bonding temperature (see Optimal bonding

    temperature). The main two effects that lower melt-back

    distance are (1) significant diffusion of the interlayer

    material into the substrate before melting (see Critical

    interlayer thickness) and (2) loss of liquid due to wetting of

    the substrate’s sides [44] or a high bonding pressure that

    squeezes liquid out [22, 44, 62, 134, 165].

    Many materials that are joined by TLP bonding have

    carefully designed microstructures to achieve certain

    mechanical properties. Too much melt-back of the sub-

    strate by the liquid interlayer can have detrimental effects

    on the final bond in addition to lengthening the isothermal

    solidification time (see Critical interlayer thickness). And,

    in some systems melt-back can reach five to fifteen times

    the original interlayer thickness [43, 121, 146]. To prevent

    drastic melt-back that can adversely affect the micro-

    structure, the interlayer should be thin [57, 62], of a

    eutectic composition [85], or of a composition similar to

    the substrate material [19].

    Solidification

    After the liquid interlayer has reached its maximum width,

    the interlayer material diffuses into the substrates at a rate

    somewhere between the diffusivity of the liquid and solid

    [25, 43, 85, 163]. As this diffusion occurs isothermally, the

    liquid region contracts (CP5b) to conserve mass as the

    solidus and liquidus concentrations are now fixed. Iso-

    thermal solidification occurs until all of the liquid has

    disappeared (CP5c). At this point, the TLP bonding process

    can be stopped if desired [71]. The bond already has an

    elevated remelting temperature (T5) compared to the

    melting temperature of the interlayer (T3).

    Homogenization

    In most cases TLP bonding is continued in order to

    homogenize the bond. This can be an extended time in the

    same heating apparatus or a post-bond heat treatment

    applied at some other time [14]. Furthermore, if the sub-

    strate material’s microstructure is extremely sensitive, this

    stage can be conducted at a lower temperature [2, 9]. In

    either case, the bond undergoes homogenization for some

    predetermined time which causes smoothing of the solute

    peak (CP5d) that remained at the end of isothermal solid-

    ification (CP5c). The resulting remelting temperature of the

    bond in this case is TR,P. If the peak concentration (c5,P) is

    within the room-temperature solid-solubility limit of the

    binary system, the precipitation of strength-reducing

    intermetallic compounds upon cooling will be avoided [12,

    110, 147, 150, 160].

    If the bond is homogenized for a sufficient amount of

    time, there is no gradient in the concentration profile

    (CP5e) and the bond’s remelting temperature is even

    higher (TR,F). However, despite the increases in bond

    remelting temperature that can be achieved by complete

    homogenization, an adequate homogenization time is

    usually determined by a sufficiently high bond strength [2,

    24, 26, 42, 83, 103, 122, 123, 146, 150] or economic

    considerations that limit furnace time [77, 125, 173].

    Nonetheless, the bond’s remelting temperature is often

    hundreds of degrees (�C) above the melting point of theinterlayer and can be about 1000 �C higher if refractorymetals such as Ir, Mo, Nb, Os, Re, Ta, or W are used as the

    Table 2 Interlayer thicknesses for TLP bonding

    Thickness

    range (lm)Common

    thickness(es) (lm)Freq.

    (%)

    References

    \1 5 [35, 103, 130]1–5 1, 2 10 [20, 21, 35, 54, 62–64, 102, 105, 107, 108, 114, 118, 129, 130, 144, 164, 165]

    10–30 20, 25 35 [5, 8, 10, 20–25, 34, 35, 39, 44, 48, 54, 59–63, 66, 68, 74–76, 78–80, 82, 87, 89, 105, 107,

    110, 117, 118, 120–123, 126, 131, 134, 137, 141–143, 145–147, 150, 152, 155, 166–171]

    40–60 50 24 [2, 5, 20, 26, 27, 32, 33, 36, 37, 40, 42, 46, 51, 52, 55–60, 64, 69–71, 77, 78, 81, 83, 84, 87,

    88, 90, 101, 115, 119, 124–128, 135, 136, 145, 148, 149, 153, 155, 157, 166, 167, 172]

    70–150 75, 100 18 [4, 5, 11, 14, 17, 18, 22, 29, 31, 38, 42–45, 49–51, 53, 78, 86, 87, 109, 125, 134, 135, 147,

    151, 155, 159, 162]

    200–500 200, 500 6 [6, 16, 55, 77, 95–97, 100, 104, 140, 158, 159, 162, 171]

    [500 2 [65, 97]

    5308 J Mater Sci (2011) 46:5305–5323

    123

  • substrate or if low melting-point metals such as Al, Ga, In,

    Mg, Pb, Sb, Sn, or Zn are used as the interlayer.

    Time frame of TLP bonding

    The time frame of TLP bonding is highly dependent on the

    material system (e.g., phase diagram particulars, diffusion

    coefficients, grain size [18, 25, 142]) and the experimental

    parameters (e.g., interlayer thickness, bonding pressure,

    bonding temperature). The duration of each discrete stage

    of TLP bonding lies within the following ranges:

    • Heating to the bonding temperature, CP1–5a: less thana minute to about an hour; dependent on the method of

    heating, the heating rate of the heating apparatus, and

    the substrate material’s thermal properties

    • Melting of the interlayer, CP3: less than a second [121,124, 138] to several seconds [19, 43, 77]

    • Melting back of the substrate, CP3–5a: seconds [11, 71,73, 77, 124, 138, 161, 174] to minutes [7, 36, 37, 43,

    71, 73, 85, 121]

    • Isothermal solidification, CP5a–5c: minutes [7, 25, 36,37, 56, 74, 77, 95, 96, 105, 121, 125, 153] to hours [7,

    11, 33, 36, 37, 43, 57, 58, 105, 146, 157, 175], although

    it can occur in less than a minute [73, 161] or take more

    than a day [12]

    • Homogenization, CP5c–5e: hours [33, 43, 88, 109, 121]to days [88, 175] or, in a few cases, minutes [73].

    The general trend is that initial melting of the interlayer

    occurs an order of magnitude faster than melting back of

    the substrate, which occurs an order of magnitude faster

    than isothermal solidification, which occurs an order of

    magnitude faster than complete homogenization. Isother-

    mal solidification ends up being the limiting, or controlling,

    time in producing a successful TLP bond [12, 36, 104, 125,

    135, 138, 166, 167]. While the homogenization stage takes

    longer if carried to completion, it rarely is. As previously

    stated, homogenization can be performed during a sub-

    sequent heat treatment or skipped in some cases; it can

    even occur once the part is in service.

    The foregoing explanation of TLP bonding kinetics also

    applies to eutectic systems when the interlayer is a eutectic

    composition alloy. The kinetics are slightly different (and

    more importantly, TLP bonding takes much longer) for a

    eutectic system when pure elements are used. (See refer-

    ences [19, 44] for particulars of eutectic system kinetics).

    Tuah-Poku et al. [43] reported a drastic decrease in time to

    isothermally solidify by changing the interlayer: 200 h

    when using the pure element as compared to 8 h when

    using the eutectic composition. This occurs because (1) the

    interlayer has to undergo a certain amount of solid-state

    diffusion with the substrate at the bonding temperature

    before any liquid appears and (2) melt-back of the substrate

    is then greater.

    Critical interlayer thickness

    During initial heating, the interlayer element diffuses into

    the substrates. The magnitude of diffusion depends upon

    the specific material combination, but all solid-state dif-

    fusion rates increase as the temperature rises. Depending

    on the heating rate and the thickness of the interlayer, the

    amount of diffusion can significantly decrease the inter-

    layer’s width. In fact, for a combination of high diffusion

    rate, slow heating, and/or thin interlayer, it is possible to

    diffuse all of the interlayer material into the substrate

    before reaching the interlayer melting point [114, 173],

    although this is a rare occurrence. Because TLP bonding

    requires the formation of a bulk liquid phase [9, 109, 114]

    to create a consolidated, void-free bond while also

    increasing diffusion rates, the interlayer must exceed a

    minimum, or critical, thickness [105, 114].

    In addition to the parameters listed above, the critical

    interlayer thickness has been shown to depend on other

    variables such as applied clamping force, solid/liquid sur-

    face tension, surface roughness of the substrate, and

    intermetallic formation [18, 94, 114]. In short, experiments

    must be conducted for each material combination to

    empirically reveal its critical interlayer thickness.

    On the other hand, analytical models of TLP bonding

    indicate that the isothermal solidification process time is

    roughly proportional to the square of the interlayer thick-

    ness [9, 18, 19, 25, 36, 44, 86, 104, 110, 114, 124, 138, 161,

    173, 175, 176]; experimental data often corroborates this

    trend [3, 26, 43, 44, 71, 86, 88, 153]. Therefore, to mini-

    mize bonding time, an interlayer slightly thicker than the

    critical thickness is ideal.

    Optimal bonding temperature

    The bonding temperature is sometimes completely limited

    by the microstructural stability of the substrate material [7,

    9, 87, 125]. If, however, the substrate material allows

    flexibility in selecting an optimized bonding temperature, a

    minimum isothermal solidification time (and therefore

    bonding time) can be achieved at a certain temperature.

    If phase diagram and diffusion data are available for the

    material system in question, the isothermal solidification

    time can be characterized with respect to temperature.

    However, it is usually the case that experiments are the

    only way to discover this relationship. In general, the

    relationship is parabolic, yielding a minimum isothermal

    solidification time at a given intermediate temperature

    (between the melting points of the interlayer and substrate

    materials) [9, 18, 43, 50, 78, 79, 159, 162]. And yet, in

    J Mater Sci (2011) 46:5305–5323 5309

    123

  • some cases the variables of the system yield either (1) a

    monotonically increasing time, in which case the optimal

    bonding temperature is just above the interlayer’s melting

    point, [6, 9, 43, 114, 158, 162] or (2) a monotonically

    decreasing time, in which case the optimal bonding tem-

    perature is as high as the substrate material allows [4, 104,

    114, 135, 141].

    The behavior of this trend is highly system dependent

    and results in part from the interplay of the diffusion rate

    and the phase diagram of the system [19, 43, 50]. As the

    temperature is increased, the rate of diffusion increases

    exponentially. In addition, intermetallic regions, which

    tend to slow down the rate of diffusion [60, 110], can often

    be avoided by raising the temperature. As shown in Fig. 2,

    Pb diffusing into Pd at 400 �C (T1) would pass through fiveintermetallic regions. T2 and T3 are ideal temperatures for

    passing through just two and one intermetallic regions,

    respectively. T4 completely avoids the intermetallic regions

    while still providing a wide solubility range for the liquid

    to solidify.

    In addition to intermetallics, the shape of the solidus and

    liquidus lines plays an important role in TLP bonding

    kinetics and the optimal bonding temperature. Figure 3

    demonstrates extremes of solidus and liquidus lines in a

    binary system with complete solid solubility. The compo-

    sition profiles below each set of phase diagrams demon-

    strate the initial melting and isothermal solidification

    behavior of the interlayer for each case. It is assumed that

    all four systems (1) have the same diffusion coefficient and

    (2) are heated instantaneously. The latter assumption is

    accurate for many material systems since complete melt-

    back often consumes much of the solute that has diffused

    into the substrate (see CP5a in Fig. 1). The top concen-

    tration profiles illustrate initial melt-back of a pure inter-

    layer—the dotted line is the initial interlayer and the solid

    line is the molten interlayer. The bottom concentration

    profiles illustrate isothermal solidification for all four sys-

    tems after a set time.

    The partition coefficient (k) is included in the diagram

    and is defined as:

    k ¼ cScL

    ð1Þ

    where cS and cL are the solidus and liquidus compositions

    of the interlayer element.

    Systems a and b in Fig. 3 have the same convex-shaped

    liquidus line and therefore experience the same amount of

    melt-back (see the top concentration profiles). The same is

    true for the concave-shaped liquidus line in systems c and

    d. Systems a and c have the same partition coefficient (0.9).

    The same is true for systems b and d (0.4).

    A few principles of TLP bonding kinetics can be

    gleaned from this figure. First, the convex-shaped liquidus

    line (a and b) prevents melt-back from occurring to a large

    extent, whereas the concave-shaped liquidus line (c and

    d) causes much more melt-back. Second, isothermal

    Fig. 2 Pb–Pd binary system[177] illustrating bonding

    temperatures (dotted lines) thatavoid intermetallic regions

    5310 J Mater Sci (2011) 46:5305–5323

    123

  • solidification occurs faster in systems with a higher parti-

    tion coefficient (a and c). To conserve mass, the volume of

    solidified liquid is equal to the change in the concentration

    profile of the solid region. The width of isothermal solid-

    ification in an arbitrary time period is equal to the ratio of

    this volume to the difference between the liquidus and

    solidus compositions, or, written another way:

    Vliq ¼ ðcL � cSÞwisoth:solidif: ð2Þ

    Although systems a and c have the same partition coeffi-

    cient, because the liquidus and solidus compositions of

    system c are closer to zero, they are also closer to each

    other, causing isothermal solidification to occur slightly

    faster (see Fig. 3).

    If the substrate material has a sensitive microstructure

    that could be damaged by significant melt-back, then phase

    diagrams such as systems c and d should be avoided.

    Systems b and d will take much longer to isothermally

    solidify, raising operating costs.

    Systems a and c are quite similar in rate of isothermal

    solidification. Because the solidus composition of system

    c is closer to the completely homogenized composition

    (shown as an x on the gray line), homogenization of the

    solute peak after isothermal solidification will likely pro-

    ceed more rapidly than in system a. However, because the

    solidus line of system a has a convex shape, increases in

    bond remelting temperature due to homogenization will

    likely occur faster and be larger in this system.

    Modeling of TLP bonding

    Analytical models have been developed by many

    researchers for the four stages of TLP bonding to provide

    quick estimates or general trends, such as those illustrated

    in the previous section. Equations for and descriptions of

    TLP bonding analytical models are included in references

    [8, 19, 162, 178]. Assumptions made for these models are

    similar to those made in this article (see TLP bonding

    kinetics). In some cases these equations provide good

    results, but for many systems these simplified, binary-

    system approaches do not supply accurate estimates [5, 8,

    38, 78, 79, 86]. This is due in part to the diffusion coeffi-

    cients being assumed independent of composition.

    Some complexities of TLP bonding are quite difficult

    to model. For example, grain boundaries can cause iso-

    thermal solidification to occur at a different rate than that

    predicted by analytical models using a bulk diffusion

    coefficient [25, 36, 37]. Indeed, grain boundary diffusion

    is faster than bulk diffusion in a certain temperature range

    (based on the alloy’s melting point) [173]. Grain bound-

    ary diffusion rates also increase as the substrate material’s

    grain size decreases [179]. Further, grain boundaries can

    be penetrated by the liquid to cause a non-planar solidi-

    fication front, thereby increasing the area over which

    diffusion occurs [5, 11, 18, 138]. See references [180,

    181] for more information on the effect of grain bound-

    aries in TLP bonding.

    T

    ci ci c i100 0 100 0 100 0 100 0c i

    a b c

    a cb d

    a cb d

    d

    ka = = 0.983.793.0

    kc = = 0.936.040.0

    kd = = 0.416.040.0

    kb = = 0.437.293.0

    ci

    c i

    c L,a

    cS,a c S,b c S,c

    c L,cc S,d

    c L,dc L,b

    c L,ac S,a

    cS,b

    cL,b

    cS,ccL,c

    cS,d

    cL,d

    Fig. 3 Four binary systems (a–d) with complete solid solubility

    and associated concentration

    profiles. These profiles illustrate

    the initial condition (dottedline), initial melt-back of thesubstrate, and resulting

    concentrations after a set

    amount of TLP bonding has

    occurred in all four systems.

    Partition coefficient values are

    also shown for all four systems

    at the given bonding

    temperature

    J Mater Sci (2011) 46:5305–5323 5311

    123

  • Another interesting deviation is that isothermal solidi-

    fication can occur in two different ‘‘regimes’’ [38, 50, 138].

    The faster solute element of a multi-component interlayer

    controls the rate of solidification for the first regime. Then,

    a second solute element controls the rate of solidification

    during the second regime, resulting in complex concen-

    tration–time profiles.

    Numerical models can account for some of the com-

    plexities of TLP bonding to accurately predict bonding

    kinetics [7, 8, 161, 162, 168, 173, 176, 179, 182, 183] and

    can even be extended to multi-component systems [174,

    184]. Despite the complexities and extra time required in

    numerical modeling, especially for multi-component sys-

    tems, the limiting factor is most often the lack of necessary

    diffusion data [7, 8, 178]. But, when the necessary data is

    available, modeling of TLP bonding can drastically reduce

    the number of experiments required to determine optimal

    bonding parameters [37, 162, 166].

    Advantages and disadvantages of TLP bonding

    The most distinctive advantage of TLP bonding is that the

    resulting bond can operate at the bonding temperature or

    higher temperatures. In other words, materials can be

    bonded at a temperature equal to or lower than what the

    assembled part will experience in service. This is espe-

    cially important for temperature-sensitive materials whose

    microstructures can be damaged by too much thermal

    energy input [117] and therefore need to be joined at lower

    temperatures.

    Another advantage is that the resulting TLP bonds often

    have microstructural, and therefore mechanical, properties

    similar to the properties of the base materials [7, 12–14, 24,

    32, 42, 49, 61, 62, 75, 77, 81, 95, 105, 109, 115, 119, 123,

    141, 149, 153, 166, 175]. In fact, in some cases the bond

    area becomes indistinguishable from other grain bound-

    aries [18, 35, 37, 68, 108, 109, 130, 185] due to significant

    diffusion at high temperature. Such bonds are often as

    strong as the bulk substrate material [14, 164], or stronger,

    causing the joined assembly to fail in the substrate material

    rather than in the bond [14, 31, 71, 76].

    Advantages of TLP bonding include:

    • the process is highly tolerant to the presence of a fayingsurface oxide layer [2, 6, 7, 11, 13, 21, 42, 47, 48, 56,

    67, 80, 93, 136, 147–149, 186] and therefore requires

    less joint preparation and no fluxing agents [11, 18, 42,

    173, 187]; in a few rare cases surface oxides are

    actually beneficial to the process [129]

    • fixturing pressures are much lower than those used inother joining processes like diffusion bonding [11, 14,

    19, 24, 25, 33, 37, 42, 43, 49, 62, 68, 78, 136, 145–149]

    • little melting of the substrate material occurs, ascompared to fusion welding processes [42, 64]

    • many joints can be fabricated in one pass [11, 147]• the liquid formed during TLP bonding fills voids on

    uneven mating surfaces, making costly finishing pro-

    cesses unnecessary [2, 14, 18, 19, 33, 49, 161]

    • overaging of temperature-sensitive materials can beavoided [80, 140, 186, 188].

    For some material systems, bond properties and per-

    formance capabilities that are difficult or impractical to

    achieve using conventional joining methods are more

    accessible [189].

    However, TLP bonding is a specialized bonding tech-

    nique that can be time-consuming and expensive compared

    to other joining methods—the time required for isothermal

    solidification and sufficient bond homogenization can be

    unfeasibly long and/or uneconomical [36, 37, 104, 141].

    TLP bonding is not always suitable, specifically in the

    following cases:

    • significant melt-back of a material with a specificallydesigned microstructure [7, 62, 141]

    • the formation of a thick layer of intermetallic com-pounds in the bond that tend to lower its strength and

    ductility [9, 36, 87, 110, 141, 146, 157, 158, 167]

    • the segregation of particles in metal matrix compositesat the joint centerline, leaving a distinct weakened band

    in the joint microstructure [19, 33, 39, 42, 54, 105].

    See reference [7] for examples of specific difficulties

    that occur in TLP bonding applications. Although many

    disadvantages of TLP bonding can be overcome by opti-

    mized bonding parameters, the optimization process often

    requires much experimentation.

    Applications of TLP bonding

    Since TLP bonding was developed, it has successfully been

    applied to join a broad range of materials and structures

    including the following:

    • Al-, Co-, Fe-, Ni-, and Ti-based alloys [7, 10, 11, 24,43, 47, 54, 65, 85, 109, 154, 173, 190, 191]

    • Cellular structures [15, 91]• Ceramics [114, 173]• Metal matrix composites [7, 54, 93, 114, 173]• Microcircuitry components [102, 104, 152, 157, 173,

    192, 193]

    • Oxide-dispersion-strengthened alloys [7, 24, 65, 125,126]

    • Single crystals [3, 65]• Stainless steels [25, 47, 54, 85, 190]• Structural intermetallics [7, 12, 47, 51, 83, 85].

    5312 J Mater Sci (2011) 46:5305–5323

    123

  • TLP bonding is often used in high-stress, high-temper-

    ature applications where brazing, welding, and diffusion

    brazing cannot be used for various reasons (e.g., low

    melting temperature bond, insufficient resulting mechani-

    cal properties, unacceptable plastic deformation) [4, 11, 12,

    14, 19, 44, 49–51, 69, 85, 86, 92, 119, 130, 136, 141, 146,

    149, 164, 186]. Specific applications are the repair of Ni-

    based superalloy turbine blade components [7, 9, 39, 74,

    104, 105, 135, 142] and the joining of heat-resistant alloys

    that are inherently susceptible to hot cracking or post-weld

    heat treatment cracking [5, 11, 20, 38, 59, 78, 80, 135, 136,

    140, 173]. Table 3 presents a spectrum of TLP bonds as of

    now, including bonds of dissimilar materials.

    Variants of TLP bonding

    A few variants of TLP bonding also exist:

    • Temperature gradient TLP bonding: the application ofa temperature gradient causes a non-planar bond

    interface which tends to result in stronger bonds [8,

    21, 164, 186, 194]

    • Wide-gap TLP bonding: gaps of 100–500 lm can bebonded or repaired by the use of a melting and a non-

    melting constituent (multiple layers or mixed powders)

    [7, 16, 57, 92, 94–96, 100, 101, 136, 149, 173, 195]. This

    technique can also be used in conventional TLP bonding

    to accelerate isothermal solidification [13, 99, 140]

    • Active TLP bonding: a ceramic and metal can be joinedby a multi-component interlayer; at least one constit-

    uent reacts with the ceramic while another diffuses into

    the metal to cause isothermal solidification [28, 42, 52,

    54, 116, 132, 196]

    • Partial TLP bonding (see next section).

    Bonds made using temperature gradient, wide-gap, and

    active TLP bonding have been included in Table 3.

    Partial transient liquid phase (PTLP) bonding

    Partial transient liquid phase (PTLP) bonding is a variant of

    TLP bonding mainly used to join ceramics. PTLP bonding

    overlaps both wide-gap and active TLP bonding, although

    articles defining PTLP bonding predate the other two

    techniques by a few years. Many advantages of conven-

    tional TLP bonding carry over to PTLP bonding [188]. The

    ensuing sections focus on how PTLP bonding differs from

    TLP bonding.

    PTLP bonding process

    In PTLP bonding, the interlayer consists of thin layers of

    low-melting-point metals or alloys on each side of a much

    thicker refractory metal or alloy layer [188, 200–203].

    Figure 4 presents a general, three-layer PTLP bond setup.

    (In some cases, there can be multiple thin layers on each

    side of the refractory core (see Table 4), but the general

    principles of the process remain the same.) Upon heating to

    the bonding temperature, a liquid is formed (through

    melting or a eutectic reaction with the refractory core

    [202–206]) by each thin layer. The liquid that is formed

    wets each ceramic substrate while concomitantly diffusing

    into the solid refractory core. As in TLP bonding, the liquid

    regions solidify isothermally and homogenization of the

    entire bond region leads to a refractory bond.

    The refractory core tends to be a foil that is 20–30 lm[143, 207–214] or 100–127 lm thick [116, 188, 189, 201,207, 211–213, 215–222], although it can be in the

    200–1000 lm range [202–205, 208, 223–225]. Therefractory core element is often Ni [144, 189, 196, 201–

    204, 207–210, 218, 224, 226, 227]; other elements (and an

    alloy) that have been used include Au, Co, Cu, Nb, Ni–Cr,

    Pd, Pt, Si, Ta, Ti, and V [117, 188, 189, 200–202, 205–208,

    214–218, 222, 227–229]. The thin layers can be most of the

    formats used for TLP bonding interlayers (see TLP bond-

    ing process) and are often in the 1–10 lm thick range. Theratio of the thin layer thickness over the refractory core

    thickness is usually 1–5% [143, 188, 189, 201–204, 207,

    208, 211–213, 215–218, 220, 222–225, 230, 231], although

    it can be 6–20% [207, 210–213, 219, 221, 223], and some

    PTLP bond experiments have utilized a ratio of 50% or

    higher [116, 144, 208, 214, 226].

    PTLP bonding kinetics

    Figures 5 and 6 depict the two ends of the PTLP bonding

    process. The following additional assumptions are made in

    this analysis: (1) thin layer A (tlA), the refractory core (rc),

    and thin layer B (tlB) are different pure elements (2) there

    is no diffusion into the ceramic substrates (3) the ternary

    system (tlA–rc–tlB) can be approximated by the two

    associated binary systems (tlA–rc and rc–tlB), and (4) the

    interlayers wet the substrate with a thin layer of interme-

    tallic formation that conserves the amount of liquid and

    results in a refractory intermetallic.

    The second and fourth assumptions highlight the major

    differences between TLP and PTLP bonding. First, the

    multi-layer interlayer used during PTLP bonding has been

    termed ‘‘self-contained’’ [215] because the liquid phases

    must diffuse into the rc, rather than the much larger sub-

    strate materials, to induce isothermal solidification. Sec-

    ond, the liquid phases must wet the ceramic substrates to

    create a strong bond. This tends to be difficult due to the

    chemical inertness of ceramics [117, 180, 196, 216] and

    usually requires the use of active elements such as Al, Cr,

    Hf, Nb, Ni, Sc, Ta, Ti, V, or Zr [65, 117, 187, 189, 198,

    J Mater Sci (2011) 46:5305–5323 5313

    123

  • Table 3 A spectrum of materials joined by TLP bonding

    Substratea Interlayer(s)b Reference(s)

    Ni-based alloys

    GTD-111 MBF-30, MBF-50 [3, 68, 79, 82]

    Inconel 600 NB 150 [135]

    Inconel 617 BNi-3, BNi-6 [147, 156]

    Inconel 625 BNi-2 [104]

    Inconel 713C BNi-6 [88]

    Inconel 718 BNi-2 [104]

    Inconel 738 NB 30, NB 150, BNi-3, MBF-60, MBF-80,

    DF-3

    [5, 38, 45, 66, 78, 80, 86,

    87, 159, 162, 178]

    Inconel MA758 Ni–B, Ni–Cr–Si–Fe–B, MBF-80 [24, 108, 125, 141]

    Inconel MA760 Ni–Cr–P, Ni–Cr–Si–Fe–B [64]

    Inconel 939 F20, F24, F25, F26, F27, MBF-80 [59]

    Mar-M247 F20, F24, F25, F26, F27, MBF-80 [59]

    Nimonic 80A Ni|NB 125|Ni [109]

    René N5 Ni–Ge, Ni–Mn, Ni–Mn–Si, D-15 [6, 16, 158]

    Udimet 700 Ni–Cr–Co–Mo–B [14]

    Waspaloy NB 150 [38, 50, 178]

    Ni–6.4Al Ni–B [157]

    Ni–15Cr–11.5Al–3 W–0.2Hf–0.1Si–0.1Mn (c/c0/b type) MBF-80, Ni–Cr–B–Ce (variouscombinations)

    [65]

    Al-based alloys

    Al A356.0 Cu [107]

    Al 5052 Ag–Cu [127]

    Al 6060 Al–Cu, Al–Si–Cu [165]

    Al 6061 Ag, Al–Si, BAg-8 [17, 27]

    Al 6082 Cu, Ga [21, 129, 164]

    Al 7475 Zn [30]

    Al–7.5Si Cu [107]

    Fe-based alloys

    304 SSc Ni–Cr, 304L SSc, BNi-2 [77, 99]

    304L SSc NB 51 [91]

    Duplex SSc Cu, Fe–B–Si, Ni–Si–B, MBF-20, MBF-30,

    MBF-35, MBF-50, MBF-80

    [25, 47, 61, 76, 153, 169]

    Carbon steel Cu, Fe–B [36, 37, 74]

    Fe–Ni–Cr Ni–B–Cr–Si (various combinations) [133]

    Incoloy MA956 B, Fe–B–Si [35, 63, 65, 130]

    Incoloy MA957 Fe–B–Si, BNi-1a, BNi-3 [62, 63, 126]

    Low carbon steel Fe–B–Si, BNi-2 [67, 75]

    ODSc steel (Fe–Cr–W–Y2O3–Ti) Fe–Si–B [131]

    PM2000 (Fe–Cr–Al) B, Fe–B–Si [35, 63, 130]

    T91 steel Fe–B–Si, Fe–Ni–Cr–Si–B, BNi-2 [60]

    Ti-based alloys

    OT4 Cu–Ti, Ni–Ti, Ti–Cu–Zr [97, 134]

    VT1 Cu [46]

    Ti–6Al–4 V Cu [34]

    Ti–22Al–25Nb (a) Ti–Cu–Ni [83]

    Miscellaneous alloys

    AZ31 (Mg–Al–Zn) Al, Cu [121, 150]

    K640 (Co–Cr–Mo) Co–Ni–Cr–W–B–Si [2]

    5314 J Mater Sci (2011) 46:5305–5323

    123

  • Table 3 continued

    Substratea Interlayer(s)b Reference(s)

    Co alloy (unspecified) Ni–Cr–B [10]

    Cu (ODSc) Cu | Sn | Cu [110, 151]

    Cu–Cr–Zr Cu | Sn | Cu [110]

    Sn–Ag Sn–Bi, Bi–Sn (various combinations) [106]

    Single crystals

    Ni Ni–P [142]

    CMSX–2 F24, MBF-80 [26, 70, 71]

    CMSX–4 D-15, MBF-80 [9, 26]

    IC 6 (with and without B) MBF-80 [53]

    PWA 1483 (Ni–Cr–Co–Ta–Ti–W–Al–Mo) Ni–Ge [6, 158]

    Intermetallics

    Ni–45Ti–6Cu Cu [32]

    NiAl Ni (glaze), BNi-3 [84, 113]

    Ti–42Al–2Cr Ti | Cu, Ti | Ni, Ti | Fe [51]

    Ti–45Al–2Nb–2Mn (a) ? 0.8 vol.% TiB2 Ti–Cu–Ni, Cu–Ni | Ti | Cu–Ni [20]

    c-TiAl [Ti–47Al–2Cr–2Nb (a)] Tini 67 [40]

    Ti–48Al–2Cr–2Nb (a) Cu, Cu & Ti–Al–Cr–Nb, Cu & TiAl [94, 96, 100, 197]

    Gamma Met PX Cu & Gamma Met [95]

    Pure metals

    Ag Cu, Ag–Cu [8, 43, 44]

    Al Ag, Cu, Ga, Al–Cu, Al–Si–Cu [22, 129, 148, 164, 165,

    186]

    Au Au–Sn, Sn, In, Ti | In [102, 152, 198]

    Cu Ag, Sn, Ag–Cu, BiIn, BiIn2, BiSn, InSn, NB

    51

    [15, 18, 44, 114, 139, 160,

    187, 192, 198]

    Fe Sb, Fe–P, Fe–B [137, 140]

    Nb Ti, Zr, V [155]

    Ni B, Cu, Hf, BNi-3, BNi-6, MBF-60, MBF-80 [4, 81, 88, 117, 138, 162,

    167, 168]

    Sn Bi [103]

    Metal matrix compositesd

    Al/Al2O3 Ag, Cu, Al–Cu, Cu–Ti [22, 42]

    Al/SiC Cu, Ni [144]

    Al 2124/SiC Ni [48]

    Al 2618/SiC Al–Ag–Cu, Al–Ag–Cu–Ti [93, 98]

    Al 6061/Al2O3 Cu [39, 105, 145, 146]

    Al 6061/SiC Cu [33, 90]

    AZ91D (Mg–Al)/TiC Al, Cu [122, 123]

    Haynes 230/Al2O3 Haynes 230 doped with B [85]

    Ti–6Al–4 V/SiC Cu–Ti–Zr [73]

    Ceramics

    Al2O3 Al, Al & SiO2, B2O3 [118, 143, 170, 199]

    SiC Ge [171]

    Si3N4 Oxynitride glass [185]

    TiO2 Bi2O3 [89]

    Dissimilar metals

    Al 7075 Ti–6Al–4 V Cu [23]

    Astroloy Mar-M247 (directionally solidified) BNi-3 [124]

    AZ31 (Mg–Al–Zn) 316L SSc Ni [120]

    J Mater Sci (2011) 46:5305–5323 5315

    123

  • 200–202, 206, 215, 216, 218, 222, 228, 232, 233]. Also,

    when analyzing the critical interlayer thickness of the thin

    layers, a portion of the liquid that forms from those thin

    layers will react with the ceramic substrate and add to the

    critical thickness.

    The PTLP bonding setup at room temperature is shown

    in Figs. 5 and 6 as concentration profiles 1A and 1B, CP1Aand CP1B, respectively. Both binary systems exhibit

    complete solid solubility. As the temperature of the bond is

    raised to the melting points of each thin layer (T4 for tlA

    Table 3 continued

    Substratea Interlayer(s)b Reference(s)

    Be Cu–Cr–Zr and Cu (ODSc) Cu | Sn | Cu [110]

    Cu Cu–W composite Al [31]

    Cu Steel BAg-8 [160]

    Cu 304 SSc Ag [10]

    Cu 304L SSc Ag [109]

    Br.Kh. (Cu–Cr) 12Kh18N10T (Fe–Cr–Ni) Cu–Mn|Ni, Cu–Ag|Ni [111]

    CMSX-4 Inconel 738 and 939 BNi-3, Niflex-110, Niflex-115 [136, 149]

    DD98 (Ni–W–Co–

    Mo–Ti–Al–Ta–Hf)

    M963 (Ni–W–Co single crystal) Ni–Cr–B [128]

    Inconel 718 Inconel X-750 BNi-2 [11]

    Mar-M247 NiAl Cu [12, 55, 57, 58]

    Mar-M247 NiAl-Hf (single crystal) Cu, NiAl & Cu, Ni3Al & Cu [55–57, 92, 101]

    Ni NiAl Cu, BNi-3 [12, 55, 57, 58, 69, 115]

    Low carbon steel Ti Cu–Mn–Ni [49]

    SSc 321 Zircaloy-4 (Zr–Sn) Ti–Zr–Cu–Ni [172]

    Steel 304L SSc Cu [160]

    TS7 (Ti alloy) 5VMTs (Nb alloy) with W, Mo, & Zr; and

    TV10 (Ta alloy) with W

    Cu–Ni [112]

    Ti–42Al–2Cr Ti 6242 Ti|Cu, Cu|Ti [29]

    Ti–6Al–4 V Ti–45Al–2Nb–2Mn (a) ? 0.8 vol.% TiB2 Cu–Ni, Ti–Cu–Ni [20]

    Metals to Metal matrix compositesd

    Al 6082 Al 359/SiC Cu [21]

    Ti–6Al–4 V Ti–6Al–4 V/SiC Cu–Ti–Zr [73]

    Metals to Ceramics

    Kovar (Fe–Ni–Co) SiC Ni–Si | Mo [116]

    ODSc Fe alloy (Fe–Cr–

    Al–Y2O3)

    Si3N4 Fe–B–Si [72]

    W18Cr4 V tool steel TiC–Al2O3 composite Cu|Ti [28]

    Inconel 718 Si3N4 Ni|Cu|Ti [196]

    Ni Ti(C,N) (50%TiC & 50%TiN) Cu|Nb [132]

    Ti AlN Ag–Cu [52]

    Metal matrix compositesd to ceramics

    Al 6061/Al2O3 Al2O3 Cu [39, 54]

    a Substrate material compositions are in weight percent, unless specified by an (a) for atomic percentb Interlayer material compositions are notated as either (1) X–Y–Z where X is the base element and Y and Z are alloying elements of at least one

    weight percent in order of descending composition or (2) one of the following braze alloy designations in weight percent: BAg-8 (Ag–28Cu),

    D-15 (Ni–15.3Cr–10.3Co–3.5Ta–3.5Al–2.3B), DF-3 (Ni–20Co–20Cr–3B–3Ta), F20 (Ni–21.6Cr–17.6Co–3.1 W–2.8Al–2.2B–1.3Ta), F24

    (Ni–10.8Co–8.8Cr–3.9 W–3Al–3Ta–2.5B), F25 (Ni–9.8Co–8.6Cr–8.2 W–2.4B), F26 (Ni–9.2Co–8.6Cr–4.9Al–3.6B–2.7Ta), F27 (Ni–9.8Co–

    7.5Cr–3.3B–1.9 W), BNi-1a (Ni–14Cr–4.5Fe–4.5Si–3B), MBF-20 or BNi-2 (Ni–7Cr–4.5Si–3.2B–3Fe), MBF-30 or BNi-3 (Ni–4.5Si–3.2B),

    MBF-35 (Ni–7.3Si–2.2B), MBF-50 (Ni–19Cr–7.3Si–1.5B), MBF-60 or BNi-6 (Ni–11P), MBF-80 (Ni–15.2Cr–4B), NB 30 (Ni–19Cr–10Si),

    NB 51 (Ni–25Cr–10P), NB 125 (Ni–14Cr–4.5Fe–4.5Si–3.13B), NB 150 (Ni–15Cr–3.5B), Niflex-110 and Niflex-115 (proprietary), Ticu-

    sil (Ag–26.7Cu–4.5Ti), Tini 67 (Ti–33Ni)c ODS oxide dispersion-strengthened, SS stainless steeld Metal matrix composites are notated as X/Y where X is the matrix material and Y is the composite fiber material

    5316 J Mater Sci (2011) 46:5305–5323

    123

  • and T3 for tlB), both thin layers diffuse into the rc (see

    CP2A and CP3A as well as CP2B). Despite the small

    amount of liquid that initially forms from tlB due to its high

    diffusivity (CP3B), the liquid drastically melts back the rc

    on further heating (CP4B) due to the concave shape of the

    liquidus. This melt-back continues until the assembly is

    heated to the bonding temperature (T5) shown in CP5aB.

    On the other hand, the liquid formed from tlA (CP4A)

    widens slightly to be about the same width as the original

    thin layer (CP5aA) due to that system’s convex liquidus.

    At this point, isothermal solidification occurs on both

    sides of the multi-layer interlayer. It proceeds much faster

    for tlB due to its high partition coefficient and diffusivity.

    In fact, isothermal solidification is complete for tlB(CP5bB) when the other liquid region has only solidified

    about halfway (CP5bA), despite the considerable melt-back

    of the rc.

    The liquid formed from tlA eventually solidifies iso-

    thermally (CP5cA). On the other side of the bond, the

    solute peak has been smoothed due to homogenization

    (CP5cB), and the remelting temperature on that side has

    increased to TR,P.

    Further homogenization causes the remaining gradient

    in the tlB element to disappear (CP5dB), thereby raising the

    thinlayer

    A

    substrateA

    substrateB

    refractorycore

    thinlayer

    B

    Fig. 4 A general PTLP bonding setup

    Table 4 A spectrum of materials joined by PTLP bonding

    Substrate Interlayera Combination(s) Reference(s)

    Ceramics

    Al2O3 Cr | Cu | Ni | Cu | Cr, Cu | Nb | Cu, Cu | Ni | Cu, Cu | Ni–Cr | Cu,

    Cu | Pt | Cu, In | Ag ABAc | In, In | Cusil ABAc | In,

    In | Incusil ABAc | In, Ni | Nb | Ni, Ti | Al | Ti

    [143, 188, 189, 201, 207, 211–213,

    215, 216, 218, 220–222, 230, 232]

    Glass Au | InBi | Au [139]

    Si3N4 Al | Ti | Al, Au | Ni–Cr | Au, Cu–Au | Ni | Cu–Au, Co | Nb | Co,

    Co | Ta | Co, Co | Ti | Co, Co | V | Co, Cu–Au–Ti | Ni | Cu–Au–Ti,

    Cu–Ti | Pd | Cu–Ti, Ni | Ti | Ni | Ti | Ni, Ni | V | Ni,

    Ti | Au | Cu | Au | Ni | Au | Cu | Au | Ti, Ti | Cu | Ti,

    Ti | Cu | Ni | Cu | Ti, Ti | Ni | Ti, Ti | Ni | 304SSc | Ni | Ti,

    Ti | Ni | Kovarc | Ni | Ti, V | Co | V

    [117, 202, 206–208, 210–212, 214,

    217, 223, 224]

    SiC C | Si | C, Cu–Au–Ti | Ni | Cu–Au–Ti, Ni–Si | Mo | Ni–Si,

    Ti | Au | Cu | Au | Ni | Au | Cu | Au | Ti

    [116, 210, 212, 213, 227]

    WC Zn | Pd | Zn [219]

    Y2O3-stabilized ZrO2 Al | Ni | Al, Ni | Nb | Ni [216, 231]

    ZrO2-toughened Al2O3 Ni | Nb | Ni [216]

    Compositesb

    Al / SiC Cu | Ni | Cu [144]

    Si3N4 / TiC Ti | Ni | Ti [203]

    Al 6061 / Al2O3 Cu | Ni | Cu [209]

    C / C Ti | Ni | Ti [226]

    Metals to ceramics

    FA-129 (Fe3Al

    alloy, Fe–Al–Cr–

    Nb)

    Si3N4 Cu–Ti (ABAc) | Cu | Cu–Ti (ABAc), Cu–Ti | Cu | Ni | Al [202, 204, 205]

    Kovarc Al2O3 Ni | Ti | Ni [200]

    Ni Si3N4 Ti | Ni | Ti [225]

    Si Al2O3 Ti | Cu | Sn | Au | Cu [229]

    a Interlayer material compositions are notated as either (1) X–Y where X is the base element and Y is the minor alloying element or (2) one of

    the following braze alloy designations, in weight percent: Cusil (Ag–28Cu), Incusil (Ag–27.3Cu–12.5In–1.3Ti), and Ticusil (Ag–26.7Cu–4.5Ti)b Composites are notated as X/Y where X is the matrix material and Y is the composite fiber materialc ABA active brazing alloy, Kovar Fe–Ni–Co alloy, SS stainless steel

    J Mater Sci (2011) 46:5305–5323 5317

    123

  • remelting temperature of the bond next to substrate B to its

    final value, TR,F. A similar melting temperature increase (to

    TR,P1) simultaneously occurs on the other side of the bond

    due to smoothing of its solute peak (CP5dA).

    Prolonging the homogenization process continues to

    raise the remelting temperature of the left side of the bond.

    However, once its remelting temperature has reached TR,P2(CP5eA), which is higher than TR,F for the right side of the

    bond, further homogenization will have little effect on

    raising the bond’s remelting temperature. From an opti-

    mization standpoint, homogenization should be stopped at

    this time. However, real-world considerations usually

    determine the homogenization time, which can be less

    than—or greater than—the optimized time due to various

    factors, such as cost, microstructural considerations, or

    resulting bond strength.

    The time frame of PTLP bonding is very similar to that

    of TLP bonding. Isothermal solidification and homogeni-

    zation times for TLP bonding depend on high-diffusivity

    elements diffusing into ‘‘infinite’’ substrate materials. In

    PTLP bonding, the elements tend to have lower diffusivi-

    ties, but the maximum diffusion path is on the order of

    100 lm, resulting in similar bonding times.

    Advantages and disadvantages of PTLP bonding

    The ‘‘self-contained’’ [215] nature of the PTLP bonding

    multi-layer interlayer provides benefits and impediments.

    Specific advantages include the following:

    • the dual nature of the multi-layer interlayer combinessome beneficial properties of brazing and diffusion

    CP5a

    CP4 CP5e

    CP3

    CP2 CP5c

    CP1 CP5brc

    L

    L

    L

    c5,Lc5,S

    c5,S

    c5,F

    c5,P1

    c5,P2

    bond region

    100 0

    T5

    TR,P2TR,F

    T4

    T3

    T2

    T1

    c5,L c5,Sc5,P2c5,P1 c5,F

    CP5f

    TR,P1

    c tlA

    s A tlAA A

    A

    CP5dA

    A

    A

    A

    A

    A

    A

    c5,Lc5,S

    Fig. 5 A schematic binarysystem with complete solid

    solubility and associated

    concentration profiles for one

    half of the PTLP bonding

    process (thin layer A [tlA] and

    refractory core). These profiles

    illustrate the thin layer A

    element’s concentration during

    the PTLP bonding process,

    starting with the initial

    condition (CP1A) and ending

    with the completely

    homogenized bond (CP5fA)

    5318 J Mater Sci (2011) 46:5305–5323

    123

  • bonding [117, 188, 204, 206, 208, 215] and provides

    some flexibility in joint design

    • lower bonding temperatures can mitigate thermallyinduced stresses [188, 214] and limit or avoid delete-

    rious intermetallic reactions [188, 207]

    • because diffusion occurs on a smaller scale (on theorder of 100 lm), bonding using slow-diffusing ele-ments occurs in a reasonable amount of time.

    Major disadvantages are:

    • the liquid interlayer must wet the ceramic [117, 143,215]

    • matching the thermal expansion coefficients of theceramic substrates and metallic interlayer elements is

    sometimes necessary to prevent thermally induced

    stresses and cracking [117, 143, 188, 196, 203, 215]

    • intermetallic formation is necessary, but a thick reac-tion layer tends to be brittle and can degrade joint

    strength [143, 200, 202, 203, 210, 215].

    However, most disadvantages of PTLP bonding can be

    overcome by proper design. In the end, the limiting factor

    is wettability on the specific ceramic material.

    Applications of PTLP bonding

    PTLP bonding has been used to successfully join some

    ceramic and composite materials. Table 4 presents a

    spectrum of PTLP bonds as of now, including bonds of

    dissimilar materials. The interlayer combination of the

    general PTLP bond setup shown in Fig. 4 would be notated

    tlA | rc | tlB.

    CP5a

    CP4 CP5e

    CP3 CP5d

    CP2 CP5c

    CP1 CP5brc s

    L

    L

    L

    c4,Lc4,S

    c5,Lc5,S

    c5,F

    c5,F

    c5,F

    c5,P

    c5,S

    bond region

    0 100

    T5

    TR,PTR,F

    T4

    T3

    T2

    T1

    c5,Lc4,L

    c5,Sc4,Sc5,Pc5,F

    CP5f

    ctlB

    tlB BB B

    B

    B

    B

    B

    B

    B

    B

    B

    Fig. 6 A schematic binarysystem with complete solid

    solubility and associated

    concentration profiles for one

    half of the PTLP bonding

    process (refractory core and thin

    layer B [tlB]). These profiles

    illustrate the thin layer B

    element’s concentration during

    the PTLP bonding process,

    starting with the initial

    condition (CP1B) and ending

    with the completely

    homogenized bond (CP5fB)

    J Mater Sci (2011) 46:5305–5323 5319

    123

  • Summary

    TLP bonding is a relatively new bonding process that

    results in a bond with a higher melting temperature than

    that used to join the materials. Specific details of this

    process, including experimental details, process kinetics,

    and optimal bonding temperature, have been outlined in

    this article. Also, the broad range of materials that have

    been joined by TLP bonding was presented.

    PTLP bonding, a more recent variant of TLP bonding

    used to bond hard-to-join materials, was also outlined.

    PTLP bonding has been successful in joining a smaller

    range of materials, most notably, ceramics.

    Both TLP and PTLP bonding are specialized joining

    processes that require more resources to implement com-

    pared to typical bonding processes. However, in some

    cases these bonding processes are the best—or only—way

    to join materials for specialized applications.

    Acknowledgements This study was funded by the Office of NavalResearch under grant number N00014-07-1-0872, Dr. William Mul-

    lins, Program Officer.

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    http://dx.doi.org/10.1007/BF00357335

    Overview of transient liquid phase and partial transient liquid phase bondingAbstractTransient liquid phase (TLP) bondingTLP bonding processTLP bonding kineticsMeltingDissolutionSolidificationHomogenization

    Time frame of TLP bondingCritical interlayer thicknessOptimal bonding temperatureModeling of TLP bondingAdvantages and disadvantages of TLP bondingApplications of TLP bondingVariants of TLP bonding

    Partial transient liquid phase (PTLP) bondingPTLP bonding processPTLP bonding kineticsAdvantages and disadvantages of PTLP bondingApplications of PTLP bonding

    SummaryAcknowledgementsReferences

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